WO2022199162A1 - Batterie au lithium-ion - Google Patents

Batterie au lithium-ion Download PDF

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Publication number
WO2022199162A1
WO2022199162A1 PCT/CN2021/140299 CN2021140299W WO2022199162A1 WO 2022199162 A1 WO2022199162 A1 WO 2022199162A1 CN 2021140299 W CN2021140299 W CN 2021140299W WO 2022199162 A1 WO2022199162 A1 WO 2022199162A1
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WO
WIPO (PCT)
Prior art keywords
lithium
ion battery
electrolyte
carbonate
mass
Prior art date
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PCT/CN2021/140299
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English (en)
Chinese (zh)
Inventor
白晶
毛冲
王霹霹
欧霜辉
黄秋洁
陈子勇
戴晓兵
Original Assignee
珠海市赛纬电子材料股份有限公司
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Publication of WO2022199162A1 publication Critical patent/WO2022199162A1/fr

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
    • H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0567—Liquid materials characterised by the additives
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • the present application belongs to the technical field of energy storage, and in particular relates to a lithium ion battery.
  • Lithium-ion batteries are widely used in 3C digital, power tools, aerospace, energy storage, power vehicles and other fields due to their high specific energy, no memory effect, and long cycle life. High battery voltage and high energy density put forward higher requirements. At present, domestic and foreign manufacturers of batteries for digital electronic products are developing in the direction of high-voltage lithium-ion batteries, and high-voltage lithium-ion batteries will have a larger market space in portable electronic devices. High-voltage lithium cobalt oxide (LCO) is currently the mainstream of 3C lithium battery cathode materials, and the market demand is rising steadily, so the output of LCO is increasing steadily year by year. The industrialization of high-voltage ( ⁇ 4.5V) LCO has pushed LCO to a new development platform.
  • LCO lithium cobalt oxide
  • the gram capacity density of LCO can be increased by 21%, which corresponds to the battery with longer battery life and better support Communication technology is upgraded from 4G to 5G or even 6G.
  • the process is accompanied by slippage between lattice layers and partial collapse of the O3 lattice structure, accompanied by an increase in the internal stress of the LCO, which further leads to LCO crack formation and particle breakage.
  • the top of the O 2- :2p resonance band overlaps with the low-spin Co 3+/4+ :t 2g resonance band, oxygen starts to undergo redox reactions at high voltages, due to the superoxide ion O 1-
  • the ion mobility is higher than that of O 2- , and the O- on the LCO surface is easily converted into O 2 and detached from the LCO particles, which will destroy the cathode-electrolyte interface, resulting in interface instability.
  • the cut-off voltage of LCO is usually lower than 4.45 V, and its limited capacity is 175 mAh/g. Therefore, slowing down the interfacial activity of LCO materials under high voltage and slowing down the decomposition of electrolyte will improve the cycle performance and storage performance of lithium-ion batteries under high voltage system.
  • the purpose of the present application is to provide a lithium ion battery, which has better cycle performance and high temperature storage performance under a high voltage system.
  • the application provides a lithium ion battery, including a positive electrode, a negative electrode and an electrolyte, the electrolyte includes a lithium salt, a non-aqueous organic solvent and an additive, the active material of the positive electrode includes lithium cobaltate, and the additive includes the structure of formula 1.
  • R 1 and R 2 are each independently selected from hydrogen, an alkali metal or a hydrocarbon group having 1-4 carbon atoms.
  • the active material of the positive electrode of the lithium ion battery of the present application includes lithium cobalt oxide
  • the electrolyte includes an additive
  • the additive includes the compound represented by the structural formula 1
  • the compound represented by the structural formula 1 is used in the positive electrode of the lithium ion battery.
  • a nitrogen-containing passivation film can be formed on the surface of the negative electrode, and the nitrogen-containing passivation film formed on the surface of the negative electrode can protect the negative electrode material and reduce the reduction and decomposition of the electrolyte, thereby improving the cycle performance of lithium-ion batteries.
  • the nitrogen-containing passivation film formed on the surface of the positive electrode can protect the positive electrode material and inhibit the transition of the O3 phase to the O1 phase when the lithium cobalt oxide material is charged to a higher voltage, thereby inhibiting the oxygen evolution of the positive electrode and reducing the oxidative decomposition of the electrolyte, thereby increasing the lithium ion
  • the cycle and high-temperature storage performance of the battery, and the compound represented by structural formula 1 can also capture hydrofluoric acid to inhibit the decomposition of the electrolyte, so it can also improve the cycle and high-temperature storage performance of the lithium-ion battery.
  • the compound represented by structural formula 1 is more stable due to its own symmetrical structure, so the compound represented by structural formula 1 has a higher oxidation potential after film formation, and is more stable at higher temperatures.
  • the nitrogen-containing organic electrolyte membrane formed under high voltage is not easily decomposed under high voltage, which can further improve the cycle performance and high-temperature storage performance of lithium-ion batteries.
  • the compound shown in the structural formula 1 of the present application is selected from at least one of compounds 1 to 6:
  • the mass of the additive of the present application accounts for 0.1-0.8% of the mass of the electrolyte. Specifically, it can be 0.1%, 0.2%, 0.5%, and 0.8%, but it is not limited to the listed numerical values, and other unlisted numerical values within the numerical range are also applicable.
  • the lithium salt of the present application is selected from lithium hexafluorophosphate (LiPF 6 ), lithium difluorophosphate (LiPO 2 F 2 ), lithium bis-oxalate borate (LiBOB), lithium difluorooxalate borate (LiODFB), difluorobisoxalate phosphoric acid Lithium (LiPF 2 (C 2 O 4 ) 2 ), Lithium Tetrafluoroborate (LiBF 4 ), Lithium Tetrafluorooxalate Phosphate (LiPF 4 (C 2 O 4 )), Lithium Bistrifluoromethanesulfonimide (LiN (SO 2 CF 3 ) 2 ), at least one of lithium bisfluorosulfonimide (Li[N(SO 2 F) 2 ), and lithium tetrafluoromalonate phosphate.
  • LiPF 6 lithium hexafluorophosphate
  • LiPO 2 F 2 lithium bis-oxa
  • the mass of the lithium salt of the present application accounts for 10-20% of the mass of the electrolyte, specifically 10%, 11%, 12%, 13%, 14%, 15%, 16%, 17%, 18% , 19%, 20%, but are not limited to the listed values, and other unlisted values within the numerical range are also applicable.
  • the non-aqueous organic solvent of the present application is selected from ethylene carbonate (EC), dimethyl carbonate (DMC), diethyl carbonate (DEC), ethyl methyl carbonate (EMC), propylene carbonate (PC) , at least one of butyl acetate (n-BA), ⁇ -butyrolactone ( ⁇ -GBL), propyl propionate (n-PP), ethyl propionate (EP) and ethyl butyrate (EB) kind.
  • the non-aqueous organic solvent is preferably ethylene carbonate (EC), diethyl carbonate (DEC) and ethyl methyl carbonate (EMC).
  • the mass of the non-aqueous organic solvent of the present application accounts for 60-80% of the mass of the electrolyte, specifically 60%, 65%, 66%, 67%, 68%, 69%, 70%, 71%, 72%, 73%, 74%, 75%, 80%, but not limited to the recited values, and other non-recited values within the numerical range are also applicable.
  • the electrolyte of the present application also includes an auxiliary agent, and the quality of the auxiliary agent accounts for 0.1-10.5% of the mass of the electrolyte;
  • the auxiliary agent is selected from 2,2,2-trifluoroethyl methyl carbonate, 2,2, 2-trifluorodiethyl carbonate, 2,2,2-trifluoroethylpropyl carbonate, vinylene carbonate (VC), fluoroethylene carbonate (FEC), diethyl pyrocarbonate (DEPC), 1,3-Propane Sultone (PS), Vinyl Sulfate (DTD), 1,2-Difluoroethylene Carbonate (DFEC), Tris(trimethylsilane) Phosphate (TMSP), Tris(tris(trimethylsilyl)phosphate) Methylsilane) phosphite (TMSPi), 4,4'-bi-1,3-dioxolane-2,2'-dione (BDC), 3,3-bisulfate vinyl ester
  • the additive can form a stable passivation film on the surface of the positive electrode, prevent the oxidative decomposition of the electrolyte on the surface of the positive electrode, inhibit the dissolution of transition metal ions from the positive electrode, improve the stability of the structure and interface of the positive electrode material, and significantly improve the high temperature of the lithium ion battery. Storage performance and cycle performance.
  • the auxiliary agent is selected from vinylene carbonate (VC), fluoroethylene carbonate (FEC), 1,3-propane sultone (PS), vinyl sulfate (DTD), tris(trimethylsilane) ) Phosphate (TMSP), Tris(trimethylsilane) phosphite (TMSPi), 4,4'-bi-1,3-dioxolane-2,2'-dione (BDC), 3, Vinyl 3-bisulfate (BDTD), 1,2-difluoroethylene carbonate (DFEC), and the content is 0.1-2%, 0.2-6%, 0.2-2%, 0.2-2%, 0.1%, respectively ⁇ 1.5%, 0.1 to 1.5%, 0.1 to 1.5%, 0.1 to 1.5%, 0.1 to 1.5%.5%.
  • VC vinylene carbonate
  • FEC fluoroethylene carbonate
  • PS 1,3-propane sultone
  • DTD vinyl sulfate
  • TMSP tris(trimethylsi
  • vinyl sulfate (DTD) is added to the electrolyte as an auxiliary agent, which can modify the components of the SEI film on the negative electrode surface of lithium ion batteries and increase the relative content of sulfur atoms and oxygen atoms, which contain lone pair electrons. , which can attract lithium ions, speed up the shuttle of lithium ions in the SEI film, and reduce the battery interface impedance, thereby effectively improving the charge and discharge performance of lithium ion batteries.
  • 1,3-Propane sultone has good film-forming properties as an auxiliary agent, which can form a large number of CEI films containing sulfonic acid groups at the positive interface, inhibit the decomposition and gas production of FEC at high temperature, and improve lithium-ion batteries.
  • the capacity loss of the first charge and discharge is beneficial to improve the reversible capacity of the lithium-ion battery, thereby improving the high-temperature performance and long-term cycle performance of the lithium-ion battery.
  • Tris(trimethylsilane) phosphate (TMSP) and tris(trimethylsilane) phosphite (TMSPi) can absorb moisture and free acid to improve the cycling performance of lithium-ion batteries.
  • the active material of the negative electrode of the present application includes natural graphite.
  • the highest charging voltage of the lithium-ion battery of the present application is 4.53V.
  • the positive electrode of the present application is composed of pure lithium cobalt oxide or doped lithium cobalt oxide.
  • ethylene carbonate, diethyl carbonate and ethyl methyl carbonate were uniformly mixed in a mass ratio of 1:1:2 to obtain 79.8 g of water organic solvent, and then 0.2 g of compound 1 was added as an additive to obtain a mixed solution.
  • the mixed solution was sealed and packaged and placed in the freezing room (-4°C) for 2 hours and then taken out.
  • a nitrogen-filled glove box O 2 ⁇ 1ppm, H 2 O ⁇ 1ppm
  • compound 7, compound 8, compound 9, compound 10 are as follows:
  • Example 1 With nickel cobalt lithium manganate ternary material Li[Ni 0.9 Mn 0.05 Co 0.05 ]O 2 as the positive electrode and natural graphite as the negative electrode, the electrolyte of Example 1 is made into a high-nickel ternary lithium ion battery with reference to the conventional lithium battery preparation method , and carry out normal temperature cycle performance, high temperature cycle performance, high temperature storage performance test, its test conditions are as follows, and the test results are as shown in Table 3:
  • Capacity retention rate discharge capacity of the last cycle / discharge capacity of the first cycle ⁇ 100%
  • DCIR boost rate DCIR of the last 50 laps / DCIR of the first lap ⁇ 100%
  • the battery was placed in an oven with a constant temperature of 45°C, charged to 4.53V with a constant current of 1C, then charged with a constant voltage until the current dropped to 0.05C, and then discharged to 3.0V with a constant current of 1C.
  • the capacity retention rate and DCIR improvement rate of the high temperature cycle were calculated by the following formulas.
  • Capacity retention rate discharge capacity of the last cycle / discharge capacity of the first cycle ⁇ 100%
  • DCIR boost rate DCIR of the last 50 laps / DCIR of the first lap ⁇ 100%
  • the formed battery was charged to 4.53V at 1C constant current and constant voltage at room temperature, the initial discharge capacity and initial battery thickness were measured, and then stored at 85°C for 8 hours and then discharged to 3.0V at 1C, and the capacity retention and recovery of the battery were measured. Capacity and battery thickness after storage. Calculated as follows:
  • Battery capacity retention rate (%) retained capacity / initial capacity ⁇ 100%;
  • Thickness swelling ratio (%) (battery thickness after storage ⁇ initial battery thickness)/initial battery thickness ⁇ 100%.
  • the formed nitrogen-containing SEI or CEI film has the function of layered protection, while Comparative Example 3 and Comparative Example 5 can only form a single nitrogen-containing SEI or CEI film because there is only one imine group. Therefore, the nitrogen-containing SEI or CEI film formed by Compound 1 to Compound 6 is compared with Comparative Example 3 and Comparative Example 5. A single nitrogen-containing SEI or CEI film is more stable.
  • Comparing Example 1, Examples 4 to 8 and Comparative Example 4 the performance of the lithium ion batteries of Example 1 and Examples 4 to 8 is better than that of Comparative Example 4, because although Compound 8 also contains a diketimine structure , but because it is not a symmetric structure, when two imine functional groups participate in the film formation, the film cannot be formed in two steps, and the resulting nitrogen-containing SEI or CEI film does not have the function of layered protection. The lower film formation stability is poor, so the performance of the lithium ion battery of Comparative Example 4 is not as good as that of Example 1 and Examples 4 to 8.
  • the nitrogen-containing protective film formed by compound 1 is not so ideal in inhibiting the H2-H3 phase transition in the high-nickel ternary cathode material at high voltage, because the H2-H3 phase transition is mainly derived from When the high nickel material is in the high lithium ion state, the Ni atoms are mixed, and the compound A shown in the structural formula 1 has little effect on the inhibition of the Ni atomic mixing, so the compound A shown in the structural formula 1 is more suitable for high voltage when used as an additive. Lithium cobaltate system.

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  • Chemical & Material Sciences (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Inorganic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Secondary Cells (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

La présente invention concerne une batterie au lithium-ion qui comprend une électrode positive, une électrode négative et un électrolyte, l'électrolyte comprenant un sel de lithium, un solvant organique non aqueux et un additif, un matériau actif de l'électrode positive comprenant de l'oxyde de cobalt et de lithium, et l'additif comprenant un composé représenté par la formule structurelle (1), dans laquelle R1 et R2 sont chacun indépendamment sélectionnés parmi l'hydrogène, un métal alcalin ou un groupe hydrocarboné ayant 1 à 4 atomes de carbone. La présente batterie au lithium-ion affiche des performances de cycle et des performances de stockage à haute température relativement bonnes dans un système à haute tension.
PCT/CN2021/140299 2021-03-25 2021-12-22 Batterie au lithium-ion WO2022199162A1 (fr)

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CN202110320304.6A CN113066975B (zh) 2021-03-25 2021-03-25 锂离子电池
CN202110320304.6 2021-03-25

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Cited By (2)

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CN116154293A (zh) * 2023-04-20 2023-05-23 河北省科学院能源研究所 一种电解液及其制备方法和应用
EP4383395A1 (fr) * 2022-12-09 2024-06-12 SK On Co., Ltd. Solution électrolytique pour batterie secondaire au lithium et batterie secondaire au lithium la comprenant

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* Cited by examiner, † Cited by third party
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CN113066975B (zh) * 2021-03-25 2022-06-17 珠海市赛纬电子材料股份有限公司 锂离子电池

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CN113066975A (zh) * 2021-03-25 2021-07-02 珠海市赛纬电子材料股份有限公司 锂离子电池

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US20150064578A1 (en) * 2013-08-30 2015-03-05 Samsung Electronics Co., Ltd. Electrolyte for lithium secondary battery and lithium secondary battery using the same
CN111326728A (zh) * 2018-12-14 2020-06-23 宁德时代新能源科技股份有限公司 锂离子电池
CN113066975A (zh) * 2021-03-25 2021-07-02 珠海市赛纬电子材料股份有限公司 锂离子电池

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP4383395A1 (fr) * 2022-12-09 2024-06-12 SK On Co., Ltd. Solution électrolytique pour batterie secondaire au lithium et batterie secondaire au lithium la comprenant
CN116154293A (zh) * 2023-04-20 2023-05-23 河北省科学院能源研究所 一种电解液及其制备方法和应用

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